SILVER AGGLOMERATION IN SAPO-5 AND SAPO-11 MOLECULAR-SIEVES

被引:23
作者
MICHALIK, J
AZUMA, N
SADLO, J
KEVAN, L
机构
[1] UNIV HOUSTON,DEPT CHEM,HOUSTON,TX 77204
[2] INST NUCL CHEM & TECHNOL,PL-03195 WARSAW,POLAND
关键词
D O I
10.1021/j100013a045
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Electron spin resonance and electron spin echo modulation (ESEM) spectroscopies have been used to study the location and coordination of silver ionic clusters and silver-alcohol adducts stabilized in gamma-irradiated Ag-SAPO-5 and Ag-SAPO-11 molecular sieves. It was found that in dehydrated samples silver ionic clusters are not stabilized in contrast to zeolites, but after exposure to methanol, ethanol, and propanol before irradiation Ag-2(+) and Ag-3(2+) are efficiently stabilized. Besides silver clusters, the formation of organosilver radicals is observed, i.e., Ag . CH2OH+. By analyzing the ESEM spectra it was shown that organosilver radicals are located in the 10-ring channels of Ag-SAPO-11 and the 12-ring channels of Ag-SAPO-5 and are coordinated by two nonequivalent methanol molecules. Ag-2(+) is located in the 6-ring channels and in SAPO-5 interacts with three equivalent CH3OH groups, whereas in SAPO-11 two methanol molecules are distinctly closer to Ag-2(+) than the third one. The higher yield and stability of Ag-2(+) in SAPO-11 is associated with the preferential location of Ag+ cations in two adjacent 6-ring channels. This increases the probability of encounter between radiation-induced mobile Ag-0 and Ag+.
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页码:4679 / 4686
页数:8
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